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Register a new userAnomalous dispersion of optical phonons at the neutral-ionic transition: Evidence from diffuse X-ray scattering
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Diffuse X-ray data for mixed stack organic charge-transfer crystals approaching the neutral-ionic phase transition can be quantitatively explained as due to the softening of the optical phonon branch. The interpretation is fully consistent with vibrational spectra, and underlines the importance of electron-phonon coupling in low-dimensional systems with delocalized electrons.
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Impulsive optical excitation can generate both coherent and squeezed phonons. The expectation value of the phonon displacement $<u_q>$ oscillates at the mode frequency for the coherent state but remains zero for a pure squeezed state. In contrast, both show oscillations in $<|u_q|^2>$ at twice the mode frequency. Therefore it can be difficult to distinguish them in a second-order measurement of the displacements, such as in first-order x-ray diffuse scattering. Here we demonstrate a simple method to distinguish squeezed from coherent atomic motion by measurement of the diffuse scattering following double impulsive excitation. We find that femtosecond optical excitation generates squeezed phonons spanning the Brillouin zone in Ge, GaAs and InSb. Our results confirm the mechanism suggested in [Nature Physics 9, 790 (2013)].
Phase competition and excitations in the one-dimensional neutral-ionic transition systems are theoretically studied comprehensively. From the semiclassical treatment of the bosonized Hamiltonian, we examine the competition among the neutral (N), ferroelectric-ionic (I$_mathrm{ferro}$) and paraelectric-ionic (I$_mathrm{para}$) states. The phase transitions between them can become first-order when the fluctuation-induced higher-order commensurability potential is considered. In particular, the description of the first-order phase boundary between N and I$_mathrm{ferro}$ enables us to analyze N-I$_mathrm{ferro}$ domain walls. Soliton excitations in the three phases are described explicitly and their formation energies are evaluated across the phase boundaries. The characters of the soliton and domain-wall excitations are classified in terms of the topological charge and spin. The relevance to the experimental observations in the molecular neutral-ionic transition systems is discussed. We ascribe the pressure-induced crossover in tetrathiafulvalene-$p$-chloranil (TTF-CA) at a high-temperature region to that from the N to the I$_mathrm{para}$ state, and discuss its consequence.
A general symmetry analysis of the optical conductivity or scattering tensor is used to rewrite the conductivity tensor as a sum of fundamental spectra multiplied by simple functions depending on the local magnetization direction. Using this formalism, we present several numerical examples at the transition metal L23 edge. From these numerical calculations we can conclude that large deviations from the magneto-optical effects in spherical symmetry are found. These findings are in particular important for resonant x-ray diffraction experiments where the polarization dependence and azimuthal dependence of the scattered Bragg intensity is used to determine the local ordered magnetization direction.
We have investigated the magnetic correlations in the candidate Weyl semimetals EuCd$_2Pn_2$, ($Pn$=As, Sb) by resonant elastic X-ray scattering (REXS) at the Eu$^{2+}$ $M_5$ edge. The temperature and field dependence of the diffuse scattering of EuCd$_2$As$_2$ provide direct evidence that the Eu moments exhibit slow ferromagnetic correlations well above the N{e}el temperature. By contrast, the diffuse scattering in the paramagnetic phase of isostructural EuCd$_2$Sb$_2$ is at least an order of magnitude weaker. The FM correlations present in the paramagnetic phase of EuCd$_2$As$_2$ could create short-lived Weyl nodes.
We present a detailed analysis of resonant inelastic scattering (RIXS) from Fe$_{1.087}$Te with unprecedented energy resolution. In contrast to the sharp peaks typically seen in insulating systems at the transition metal $L_3$ edge, we observe spectra which show different characteristic features. For low energy transfer, we experimentally observe theoretically predicted many-body effects of resonant Raman scattering from a non-interacting gas of fermions. Furthermore, we find that limitations to this many-body electron-only theory are realized at high Raman shift, where an exponential lineshape reveals an energy scale not present in these considerations. This regime, identified as emission, requires considerations of lattice degrees of freedom to understand the lineshape. We argue that both observations are intrinsic general features of many-body physics of metals.
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